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Journal of Physics B Atomic Molecular and Optical Physics

Liouville-spaceR-matrix-Floquet description of atomic radiative processes involving autoionizing states in the presence of intense electromagnetic fields

V. L. Jacobs, Philip George Burke, R. M. Potvliege

Published Jan 8, 2014• 1 citation
Publisher

Abstract

A reduced-density-operator description is developed for coherent optical phenomena in many-electron atomic systems, utilizing a Liouville-space, multiple-mode Floquet–Fourier representation. The Liouville-space formulation provides a natural generalization of the ordinary Hilbert-space (Hamiltonian) R-matrix-Floquet method, which has been developed for multi-photon transitions and laser-assisted electron–atom collision processes. In these applications, the R-matrix-Floquet method has been demonstrated to be capable of providing an accurate representation of the complex, multi-level structure of many-electron atomic systems in bound, continuum, and autoionizing states. The ordinary Hilbert-space (Hamiltonian) formulation of the R-matrix-Floquet method has been implemented in highly developed computer programs, which can provide a non-perturbative treatment of the interaction of a classical, multiple-mode electromagnetic field with a quantum system. This quantum system may correspond to a many-electron, bound atomic system and a single continuum electron. However, including pseudo-states in the expansion of the many-electron atomic wave function can provide a representation of multiple continuum electrons. The 'dressed' many-electron atomic states thereby obtained can be used in a realistic non-perturbative evaluation of the transition probabilities for an extensive class of atomic collision and radiation processes in the presence of intense electromagnetic fields. In order to incorporate environmental relaxation and decoherence phenomena, we propose to utilize the ordinary Hilbert-space (Hamiltonian) R-matrix-Floquet method as a starting-point for a Liouville-space (reduced-density-operator) formulation. To illustrate how the Liouville-space R-matrix-Floquet formulation can be implemented for coherent atomic radiative processes, we discuss applications to electromagnetically induced transparency, as well as to related pump–probe optical phenomena, and also to the unified description of radiative and dielectronic recombination in electron–ion beam interactions and high-temperature plasmas.

DOI
10.1088/0953-4075/47/2/025401

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A reduced-density-operator description is developed for coherent optical phenomena in many-electron atomic systems, utilizing a Liouville-space, multiple-mode Floquet–Fourier representation. The Liouville-space formulation provides a natural generalization of the ordinary Hilbert-space (Hamiltonian) R-matrix-Floquet method, which has been developed for multi-photon transitions and laser-assisted electron–atom collision processes. In these applications, the R-matrix-Floquet method has been demonstrated to be capable of providing an accurate representation of the complex, multi-level structure of many-electron atomic systems in bound, continuum, and autoionizing states. The ordinary Hilbert-space (Hamiltonian) formulation of the R-matrix-Floquet method has been implemented in highly developed computer programs, which can provide a non-perturbative treatment of the interaction of a classical, multiple-mode electromagnetic field with a quantum system. This quantum system may correspond to a many-electron, bound atomic system and a single continuum electron. However, including pseudo-states in the expansion of the many-electron atomic wave function can provide a representation of multiple continuum electrons. The 'dressed' many-electron atomic states thereby obtained can be used in a realistic non-perturbative evaluation of the transition probabilities for an extensive class of atomic collision and radiation processes in the presence of intense electromagnetic fields. In order to incorporate environmental relaxation and decoherence phenomena, we propose to utilize the ordinary Hilbert-space (Hamiltonian) R-matrix-Floquet method as a starting-point for a Liouville-space (reduced-density-operator) formulation. To illustrate how the Liouville-space R-matrix-Floquet formulation can be implemented for coherent atomic radiative processes, we discuss applications to electromagnetically induced transparency, as well as to related pump–probe optical phenomena, and also to the unified description of radiative and dielectronic recombination in electron–ion beam interactions and high-temperature plasmas.
Liouville-space (reduced-density-operator) descriptions are developed for resonant and coherent electromagnetic interactions of quantized electronic systems, taking into account environmental decoherence and relaxation phenomena. Applications of interest include electromagnetically-induced transparency and related pump-probe optical phenomena in many-electron atomic systems (in electron-ion beam interactions, gases, and high-temperature plasmas) and semiconductor materials (bulk crystals and nanostructures). Time-domain (equation-of-motion) and frequency-domain (resolvent-operator) formulations are developed in a unified manner. The standard Born (lowest-order perturbationtheory) and Markov (short-memory-time) approximations are systematically introduced within the framework of the general non-perturbative and non-Markovian formulations. A preliminary semiclassical description of the entire electromagnetic interaction is introduced. Compact Liouville-space operator expressions are derived for the linear and the general (n'th order) non-linear electromagnetic-response tensors occurring in a perturbation-theory treatment of the semiclassical electromagnetic interaction. These expressions can be evaluated for coherent initial electronic excitations and for the full tetradic-matrix form of the Liouville-space self-energy operator representing the environmental interactions in the Markov approximation. Intense-field electromagnetic interactions are treated by means of an alternative, non-perturbative method, which is based on a Liouville-space Floquet-Fourier representation of the reduced density operator. Electron-electron quantum correlations are treated by the introduction of a cluster decomposition of the reduced density operator and a coupled hierarchy of reduced-density-operator equations.
Reduced density matrix descriptions are developed for linear and non-linear electromagnetic interactions of moving atomic systems, taking into account applied magnetic fields. Atomic collision processes are treated as environmental interactions. Applications of interest include electromagnetically induced transparency and related pump-probe optical phenomena in atomic vapors. Time-domain (equation-of-motion) and frequency-domain (resolvent-operator) formulations are developed in a unified manner. The standard Born (lowest-order perturbation-theory) and Markov (short-memory-time) approximations are systematically introduced within the framework of the general nonperturbative and non-Markovian formulations. A preliminary semiclassical treatment of the electromagnetic interaction is introduced. However, the need for a fully quantum mechanical approach is emphasized. Compact Liouville-space operator expressions are derived for the linear and the general (n'th order) non-linear electromagnetic-response tensors occurring in a perturbation-theory treatment of the electromagnetic interaction. These expressions can be evaluated for coherent initial atomic excitations and for the full tetradic-matrix form of the Liouville-space self-energy operator representing the environmental interactions in the Markov approximation. Intense-field electromagnetic interactions can be treated by means of an alternative method, which is based on a Liouville-space Floquet representation of the reduced density operator. Collisional interactions between atoms in a vapor can be treated in various approximations for the self-energy operator and the influence of Zeeman coherences on the electromagnetic response can be incorporated.
Reduced density matrix descriptions are developed for linear and non-linear electromagnetic interactions of moving atomic systems, taking into account applied magnetic fields as well as atomic collisions together with other environmental decoherence and relaxation processes. Applications of interest include electromagnetically induced transparency and related pump-probe optical phenomena in warm atomic vapors. Time-domain (equation-of-motion) and frequency-domain (resolvent-operator) formulations are developed in a unified manner. The standard Born (lowestorder perturbation-theory) and Markov (short-memory-time) approximations are systematically introduced within the framework of the general non-perturbative and non-Markovian formulations. A preliminary semiclassical treatment of the electromagnetic interaction is adopted. However, the need for a fully quantum mechanical approach is emphasized. Compact Liouville-space operator expressions are derived for the linear and the general (n'th order) non-linear macroscopic electromagnetic-response tensors occurring in a perturbation-theory treatment of the semiclassical electromagnetic interaction. These expressions can be evaluated for coherent initial atomic excitations and for the full tetradic-matrix form of the Liouville-space self-energy operator representing the environmental interactions in the Markov approximation. Collisional interactions between atoms can be treated in various approximations for the selfenergy operator, and the influence of Zeeman coherences on the macroscopic electromagnetic response can be investigated.
Linear and nonlinear (especially coherent) electromagnetic interactions of moving many-electron atoms are investigated using a reduced-density-matrix description, which is applied to electromagnetically induced transparency and related resonant pump-probe optical phenomena. External magnetic fields are included on an equal footing with the electromagnetic fields and spin-Zeeman interactions are taken into account. Complimentary time-domain (equation-of-motion) and frequency-domain (resolvent-operator) formulations of the reduced-density-matrix description are self-consistently developed. The general nonperturbative and non-Markovian formulations provide a fundamental framework for systematic evaluations of corrections to the standard Born (lowest-order-perturbation) and Markov (short-memory-time) approximations. The macroscopic electromagnetic response is described semiclassically, employing a perturbation expansion of the reduced-density operator in powers of the classical electromagnetic field. Our primary results are compact Liouville-space operator expressions for the linear and general (nthn\text{th}nth-order) nonlinear macroscopic electromagnetic-response tensors, which can be evaluated for nonlocal and nonstationary optical media described by multilevel atomic-system representations. Interactions among atoms and with environmental photons are treated as line-broadening effects by means of a general Liouville-space self-energy operator, for which the tetradic-matrix elements are explicitly evaluated in the diagonal, lowest-order, and Markov approximations. The compact Liouville-space operator expressions that are derived for the macroscopic electromagnetic-response tensors are introduced into the dynamical description of the electromagnetic-field propagation. It is pointed out that a quantized-electromagnetic-field approach will be required for a fully self-consistent quantum-mechanical treatment of local-field effects and radiative corrections.
Reduced density matrix descriptions are developed for linear and non-linear interactions in electromagnetically induced transparency and related pump-probe optical phenomena involving moving atomic systems. Applied magnetic fields as well as atomic collisions, together with other environmental decoherence and relaxation processes, are taken into account. Time-domain (equation-of-motion) and frequency-domain (resolvent-operator) formulations are developed in a unified manner. The standard Born (lowest-order perturbation-theory) and Markov (short-memory-time) approximations are systematically introduced within the framework of the general non-perturbative and non-Markovian formulations. A preliminary semiclassical treatment of the electromagnetic interaction is adopted. However, the need for a fully quantum mechanical approach is emphasized. Compact Liouville-space operator expressions are derived for the linear and the general (n'th order) non-linear macroscopic electromagnetic-response tensors within the framework of a perturbation-theory treatment of the semiclassical electromagnetic interaction. These expressions can be evaluated for coherent initial atomic excitations and for the full tetradic-matrix form of the Liouville-space self-energy operator representing the environmental interactions in the Markov approximation. Collisional interactions between atoms can be treated in various approximations for the self-energy operator, and the influence of Zeeman coherences on the electromagnetic-pulse propagation can be investigated.
A reduced-density-matrix description is developed for linear and non-linear electromagnetic interactions of quantized electronic systems in the presence of environmental decoherence and relaxation phenomena. Applications of interest include many-electron atomic systems (in electron-ion beam interactions, gases, and high-temperature plasmas) and semiconductor materials (bulk crystals and nanostructures). Time-domain (equation-of-motion) and frequency-domain (resolvent-operator) formulations are developed in a unified manner. The standard Born (lowest-order perturbation-theory) and Markov (short-memory-time) approximations are systematically introduced within the framework of the general non-perturbative and non-Markovian formulations. A preliminary semiclassical treatment of the electromagnetic interaction is introduced. Compact Liouville-space operator expressions are derived for the linear and the general (n’th order) non-linear electromagnetic-response tensors, allowing for coherent initial electronic excitations and for the full tetradic-matrix form of the Liouville-space self-energy operator representing the environmental interactions. It is emphasized that quantum-coherent many-body interactions cannot be adequately treated as environmentally induced phenomena.